Resolving Atmospheric Oxygenated Organic Molecules in Urban Beijing Using Online Ultrahigh-Resolution Chemical Ionization Mass Spectrometry DOI
Yi Yuan, Xin Chen, Runlong Cai

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 27, 2024

Gaseous oxygenated organic molecules (OOMs) are crucial precursors of atmospheric aerosols. OOMs in urban atmospheres have complex compositions, posing challenges to understanding their formation, evolution, and influences. In this study, we identify 2403 gaseous Beijing using online nitrate-based chemical ionization Orbitrap mass spectrometry based on one-year measurements. We find that can be identified with higher accuracy wider coverage, compared previously used spectrometry. With optimized OOM resolving capabilities, previous knowledge expanded. First, clear homologous oxygen-addition characteristics the revealed. Second, lower concentrations or masses characterized high confidence, e.g., above 350 Da. particular, dimers (e.g., C

Language: Английский

Cloud response to co-condensation of water and organic vapors over the boreal forest DOI Creative Commons
Liine Heikkinen, Daniel G. Partridge, Sara M. Blichner

et al.

Atmospheric chemistry and physics, Journal Year: 2024, Volume and Issue: 24(8), P. 5117 - 5147

Published: April 30, 2024

Abstract. Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance number aerosol particles that activate form droplets. The boreal forest is an important source biogenic vapors, but role these co-condensation not systematically investigated. In this work, environmental conditions under which strong co-condensation-driven droplet enhancements would be expected over biome are identified. Recent measurement technology, specifically Filter Inlet Gases and AEROsols (FIGAERO) coupled iodide-adduct chemical ionization mass spectrometer (I-CIMS), utilized construct volatility distributions atmospheric organics. Then, a suite CPM initialized comprehensive set concurrent observations collected Finland during spring 2014 performed. degree impacts formation dependent on initialization temperature, relative humidity, updraft velocity, size distribution, concentration, distribution. predicted median concentration (CDNC) due accounting organics fall average between 16 % 22 %. This corresponds activating 10–16 nm smaller dry diameter otherwise remain as interstitial aerosol. highest CDNC (ΔCDNC) presence nascent ultrafine mode geometric mean ∼ 40 no clear Hoppel minimum, indicative pristine environments (e.g., via new particle processes). Such observed 30 %–40 time studied environment when frequency highest. To evaluate frequencies such experienced by Earth system whole biome, 5 years UK System Model (UKESM1) further used. substantially lower than those at site (< 6 time), positive values, peaking spring, modeled only Fennoscandia western parts Siberia. Overall, similarities limited, limit ability model, or any similar representation, project climate relevance forest. For critical distribution regime, ΔCDNC sensitive concentrations semi-volatile some intermediate-volatility compounds (SVOCs IVOCs), especially overall surface area low. magnitudes less affected more volatile formic acid extremely low- low-volatility (ELVOCs LVOCs). reasons most condense inefficiently their high below base, LVOCs ELVOCs too low gain significant soluble reduce supersaturations enough activation occur. A reduction supersaturation caused emerges main driver ΔCDNC. results highlight potential significance close sources fresh particles. accurate predictions effects CDNC, also larger-scale models, representation critical. Further studies targeted finding observational evidence constraints field encouraged.

Language: Английский

Citations

1

Extending the Range of Detectable Trace Species with the Fast Polarity Switching of Chemical Ionization Orbitrap Mass Spectrometry DOI Creative Commons
Runlong Cai, Joona Mikkilä,

Anna Bengs

et al.

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(21), P. 8604 - 8612

Published: May 1, 2024

Chemical ionization (CI) atmospheric pressure interface mass spectrometry is a unique analytical technique for its low detection limits, softness to preserve molecular information, and selectivity particular classes of species. Here, we present fast polarity switching approach highly sensitive online analysis wide range trace species in complex samples using selective CI chemistries high-resolution spectrometry. It achieved by successfully coupling multischeme chemical inlet (MION) an Orbitrap Fourier transform spectrometer. The capability flexibly combine from both polarities effectively extends the detectability compared only one chemistry, as commonly used positive negative reagent ions tend be different We tested performance MION-Orbitrap reactive gaseous organic generated α-pinene ozonolysis environmental chamber standard mixture 71 pesticides. Diethylammonium nitrate are polarities. show that with resolving power 280,000, can switch measure within 1 min, which sufficiently stable follow temporal evolution thermal desorption profile detected 23 pesticides ion. Facilitated switching, also 47 diethylammonium, improving total number 59. For ozonolysis, combining diethylammonium addresses need oxygenated molecules environments oxidation states. These results indicate promisingly serve versatile tool nontargeted various applications.

Language: Английский

Citations

1

Gas-Phase Photolysis and Photo-Oxidation of Isoprene-Derived Atmospherically Relevant Hydroxy Nitrates DOI

Rulan Verma,

Imad Zgheib,

S. Perrier

et al.

ACS ES&T Air, Journal Year: 2024, Volume and Issue: 1(8), P. 848 - 859

Published: May 21, 2024

Volatile organic compounds (VOCs), released from both natural and anthropogenic activities, undergo oxidation in the atmosphere to form alkyl peroxy radicals (RO2) that, through subsequent chemistry, a variety of oxygenated species that may impact air quality climate. Among potential formed are nitrates (ON) can be transported over long distances contribute ozone production particle formation. The atmospheric lifetime an ON is influenced by its molecular structure. structure impacts further gas phase reaction (e.g., photolysis photo-oxidation with OH radical reaction) gas-to-particle partitioning result multiphase chemistry hydrolysis) secondary aerosol (SOA) This study investigates two atmospheric-relevant ON, specifically, hydroxy nitrates, 2-methyl-1-nitrooxy-3-buten-2-ol (C5H9NO4, -ONO2, C5-ON), 3-methyl-2-nitrooxy-4-penten-3-ol (C6H11NO4, tertiary C6-ON). Significant differences their reactivity demonstrated, C5-ON underwent faster photolysis, while C6-ON was more resistant whereas degradation during OH-initiated photo-oxidation. These attributed presence extra methyl group on C6-ON. Furthermore, products demonstrate complexity processes were detected chemical ionization Orbitrap mass spectrometry operated negative mode. Notably, cleavage O–N bond alkoxy dominant pathway addition followed RO2 bimolecular reactions (i.e., + or HO2) oxidation. research sheds light intricate atmosphere, emphasizing role fate.

Language: Английский

Citations

1

Extreme Heat and Wildfire Emissions Enhance Volatile Organic Compounds: Insights on Future Climate DOI Creative Commons
Christian Mark Salvador, Jeffrey D. Wood,

Emma Grace Cochran

et al.

Published: June 27, 2024

Abstract. Climate extremes are projected to cause unprecedented deviations in the emission and transformation of volatile organic compounds (VOCs), which trigger feedback mechanisms that will impact atmospheric oxidation formation aerosols clouds. However, response VOCs future conditions such as extreme heat wildfire events is still uncertain. This study explored modification mixing ratio distribution several anthropogenic biogenic a temperate oak–hickory–juniper forest increased temperature transported biomass burning plumes. A chemical ionization mass spectrometer was deployed on tower at height 32 m rural central Missouri, United States, for continuous situ measurement from June August 2023. The maximum observed region 38 °C, during multiple episodes remained above °C hours. Biogenic isoprene monoterpene followed closely daily profile but varying rates, whereas were insensitive elevated temperature. During period, emissions site substantially ratios acetonitrile benzene, produced biomass. An in-depth analysis spectra revealed more than 250 minor compounds, formamide methylglyoxal. overall volatility, O:C, H:C extended list responded changes presence combustion Multivariate also clustered into five factors, highlighted sources unaccounted-for VOCs. Overall, results here underscore imminent effect VOC variability, important understanding interactions between climate chemistry.

Language: Английский

Citations

1

Resolving Atmospheric Oxygenated Organic Molecules in Urban Beijing Using Online Ultrahigh-Resolution Chemical Ionization Mass Spectrometry DOI
Yi Yuan, Xin Chen, Runlong Cai

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 27, 2024

Gaseous oxygenated organic molecules (OOMs) are crucial precursors of atmospheric aerosols. OOMs in urban atmospheres have complex compositions, posing challenges to understanding their formation, evolution, and influences. In this study, we identify 2403 gaseous Beijing using online nitrate-based chemical ionization Orbitrap mass spectrometry based on one-year measurements. We find that can be identified with higher accuracy wider coverage, compared previously used spectrometry. With optimized OOM resolving capabilities, previous knowledge expanded. First, clear homologous oxygen-addition characteristics the revealed. Second, lower concentrations or masses characterized high confidence, e.g., above 350 Da. particular, dimers (e.g., C

Language: Английский

Citations

1